JP2006046646A - Low-pressure storage and deliver system for gas - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide storage and deliver systems capable of improving the delivery and the purity of supplied gas by allowing rapid fill and delivery of gases reversibly stored in a nonvolatile liquid medium. <P>SOLUTION: This low-pressure storage and delivery system for gas includes a container 4 having an interior portion containing a reactive Lewis basic or Lewis acidic reactive liquid medium 6 reversibly reacted with a gas 8 having opposing Lewis acidity or basicity, a system for transferring energy into or out of the reactive liquid medium, or a product gas purifier (e.g. a gas/liquid separator) or both. <P>COPYRIGHT: (C)2006,JPO&NCIPI

Description

  Many processes in the semiconductor industry require a reliable source of process gases for a variety of applications. Often these gases are stored in cylinders or containers and then delivered to the process under controlled conditions from the cylinder. The semiconductor manufacturing industry uses a number of harmful special gases, such as phosphine, arsine, and boron trifluoride, for example, doping, etching, and thin film deposition. These gases present significant safety and environmental challenges due to their high toxicity and pyrophoric properties (spontaneous combustibility in air). In addition to toxic factors, many of these gases are compressed and liquefied for storage in cylinders under high pressure. Storing toxic gases under high pressure in metal cylinders is often unacceptable due to the possibility of cylinder leakage or catastrophic rupture.

  Low pressure storage and delivery systems have been developed that adsorb these gases onto a solid support. Gas storage and delivery systems that are sorbed on solid sorbents are not without these problems. They suffer from inadequate capacity and delivery limits and poor thermal conductivity.

  The following patent documents and articles illustrate low pressure, low flow gas storage and delivery systems.

U.S. Patent No. 4744221, the adsorption of AsH ₃ in the zeolite is disclosed. If desired, at least some AsH ₃ is released from the delivery system by heating the zeolite to a temperature of about 175 ° C. or less. Since a significant amount of AsH ₃ in the vessel is bound to the zeolite, the effects of unintentional release due to rupture or failure are minimized compared to a pressurized vessel.

  US Pat. No. 5,518,528 discloses a physical sorbent based delivery system for storing and delivering hydrides, halides, and organometallic Group V gaseous compounds at subatmospheric pressures. ing. The gas is desorbed by delivering it to a process or device that operates at a lower pressure.

  U.S. Pat. No. 5,917,140 discloses a storage and delivery device for dispensing a sorbable fluid from a solid sorbent, each of which is adjacent to the heat of the vessel wall. Associated with enhanced heat transfer means incorporating radially extending arms to ensure a conductive relationship.

  WO 0211860 discloses a system for storage and delivery of sorbed fluid in which the fluid is retained in the sorption medium and the desorption of the fluid from the medium is facilitated by applying energy to the medium. Has been. Methods of applying energy include application of chemical potential differences to thermal energy, light energy, particle collisions, mechanical energy, and sorbed fluid.

  U.S. Pat. No. 6,101,816 discloses a fluid storage and distribution system for the liquid that distributes the vapor. Associated with the system is a fluid flow port and a fluid distribution assembly associated with the port. The assembly includes a fluid pressure controller and a flow control valve. Before the gas from within the container flows through the flow control element, it is first allowed to flow through the controller.

US Pat. No. 4,744,221 US Pat. No. 5,518,528 US Pat. No. 5,917,140 WO0211860 pamphlet US Pat. No. 6,101,816

  The present invention is directed to improvements in storage and delivery systems that enable rapid filling and delivery of gases reversibly stored in non-volatile liquid media, and improvements in the purity of delivery and delivery gases. To do.

Low pressure storage and delivery system for gas
A container having an internal portion containing a Lewis base or Lewis acid reactive liquid medium that reversibly reacts with an opposite Lewis acid or basic gas;
A system for transferring energy to or from the reactive liquid medium, or
Product gas purifier (eg, gas / liquid separator), or both,
including.

Significant advantages can be achieved by storing and delivering Lewis base or Lewis acid gas in a reactive liquid or liquid medium containing the opposite Lewis acidic or basic reactive compound. These systems consist of a container of reactive liquid medium that reacts with the gas to be stored. These systems have the following characteristics:
The ability to shorten the time required to fill the system,
The ability to eliminate and reduce liquid entrainment in the feed gas, and the gas delivered from the system if the source gas contains impurities, especially non-reactive or less reactive than the source gas The ability to increase the purity of
Have

  Storage and delivery systems based on the concept of reacting Lewis base and Lewis acid gas in the opposite acidic or basic liquid medium are unique compared to low pressure storage and delivery systems using solid absorbents or solid adsorbents. Was found to raise the problem. One of the major problems is to increase the rate at which gas can be filled into a storage and delivery system containing a reactive liquid medium, such as an ionic liquid. The term “reactive liquid medium” includes reactive liquids, solutions, dispersions, and suspensions. Another problem is increasing the gas delivery rate. Another problem is to increase the purity of the gas delivered from the storage and delivery system and to prevent the liquid from contaminating the gas delivered from the storage and delivery system during delivery. Related to that.

  To facilitate an understanding of the storage and delivery system, reference is made to the drawings. (The same number is used in the figure to represent the same component in the system apparatus.)

  FIG. 1 shows a Lewis base or Lewis acid reactive liquid medium 6 that reacts reversibly with a gas 8 (shown as bubbles) having a Lewis acidity or basicity opposite to that of the reactive liquid medium. 1 shows a gas storage and delivery system 2 composed of a container 4 containing The container 4 is equipped with a valve 10 that allows introduction of gas and liquid into the container or delivery of gas or removal of the reactive liquid medium 6. An outlet port 12 is used to deliver gas 8 from the container 4. A product gas purifier 9 is mounted above the liquid level 16 to prevent liquid from being discharged from the top space 18 with the gas through the outlet port 12 and / or to remove gas phase impurities from the gas. The product gas purifier 9 can be a gas purifier based on an adsorbent. Preferably, the product gas purifier 9 is a gas / liquid separator. The product gas purifier 9 can be composed of a membrane and a suitable membrane assembly. In some cases, the product gas purifier 9 may be disposed outside the container. The container 4 may be a cylinder generally used for compressed gas. Alternatively, the container 4 can have other shapes including a rectangular parallelepiped.

  As mentioned above, one of the problems in filling the storage and delivery system with reactive gas is the long time required to fill the container 4. It may be limited by the mass transfer (ie diffusion) rate of the gas 8 in the reactive liquid medium 6. This mass transfer process can be slow and may require days or even weeks to fill the container. To overcome mass transfer limitations, energy is added to and / or removed from the liquid during the gas filling process. By performing energy transfer, the mass transfer rate is increased via convective motion in the liquid and / or by increasing the area of the gas-liquid interface.

  One method for increasing energy transfer and hence filling rate is described with reference to FIG. In this embodiment, the inlet port 11 of the valve 10 communicates with the sparger tube 20. The term “sparger tube” is intended to encompass any type of tube capable of introducing gas below the surface of the reactive liquid medium. The sparger tube 20 can be a hard tube or a soft tube. An optional porous frit 22 having micropores of 0.1 to 500 microns is added to the outlet end of the sparger tube 20. The porous frit can be made of either metal (eg, stainless steel) or plastic (eg, polytetrafluoroethylene). The gas is then introduced through the inlet port 11 of the valve 10 and then through the sparger tube 20, which is dispersed as fine bubbles as it passes through the porous frit 22. Finely dispersed gas bubbles can more easily form complexes with reactive liquid media.

A raw material gas purifier 23 can be used to fill the container 4 with gas. The purifier outlet 24 is connected to the inlet port 11. The source gas flows into the purifier, exits from the outlet 24 and enters the container 4. The purification of the source gas results in a higher purity gas delivered from the container 4. The raw material gas purifier 23 can utilize adsorption purification, absorption purification, separation based on relative volatility difference, or reaction purification. The source gas purifier 23 is particularly effective when impurities in the source gas react with or dissolve in the reactive liquid medium. For example, the Lewis acid gas can consist of boron trifluoride (BF ₃ ) containing carbon dioxide (CO ₂ ) as an impurity. The purifier can utilize a zeolite that has a higher affinity for CO ₂ compared to BF ₃ . For example, 5A zeolite or sodium mordenite zeolite can be used. After purification, BF ₃ preferably contains less than 1 ppm CO ₂ and is charged into the container 4.

  The container 4 can also include a bubble nucleation enhancer 25. The term “bubble nucleation enhancer” is defined as any medium that serves to promote nucleation of gas bubbles. Examples of suitable nucleation enhancers include boiling tips or boiling stones, including those comprised of polytetrafluoroethylene (PTFE), microporous carbon, alumina, perforated glass, and porous metals and plastics. . The porous frit 22 can also serve as a nucleation enhancer. These nucleation enhancers increase the gas delivery rate from the vessel.

  It is also possible to remove impurities in the container 4 with the purification medium 26. This purification medium can be placed in the reactive liquid medium 6 to remove impurities. The purification medium 26 can comprise a physical adsorbent or a chemical sorbent. The chemisorbent can be a solid or it can be dissolved in a liquid medium. Examples of physical adsorbents include zeolite and activated carbon.

  The container 4 can be operated either horizontally or vertically. The liquid level should be selected so that the product gas purifier 9 is located above the liquid surface.

  FIG. 2 illustrates a less preferred method for energizing or removing energy from the reactive liquid medium 6. In the embodiment of FIG. 2, a heating mandrel 29 or a cooling mandrel 28 or both can be provided to induce convection in the reactive liquid medium 6. By heating the bottom of the container 4, the warm liquid flows upward, cools as it approaches the top surface, and then returns to the bottom of the container. This convective motion will increase the mass transfer rate and reduce the time required to fill the container with gas. The cooling mandrel 28 can be used in the same manner as the heating mandrel 29 to induce convection in the reactive liquid medium 6. The heating mandrel 29 may be placed around the surface of the container 4 (as shown in FIG. 2), or the container 4 may be placed on the heating mandrel 29. The heating mandrel 29 can be a heating blanket, a hot plate, or other suitable means for applying heat to the container 4. Alternatively, stirring by the stirrer 30 can be used to increase the heat transfer rate in the reactive liquid medium 6 and also to increase the mass transfer rate in the reactive liquid medium during filling. . An alternative means for stirring the liquid is to move the entire container 4. This can be done using standard cylinder rollers, orbital stirrers, shakers and the like. The inlet port 11 does not use the same passage as the product gas purifier 9 or the outlet 12, but rather has another passage that terminates at the inlet orifice 31 so as to bypass the product gas purifier 9 during the filling operation.

  3-5 are presented to illustrate various approaches for performing gas purification during gas delivery when the container is in a vertical or horizontal position. In particular, FIGS. 3-5 show an embodiment where the product gas purifier is a gas / liquid separator. In FIG. 3, the outlet port 12 of the valve 10 is connected to a flexible tube 36 that terminates in a porous member 37 that serves as a product gas purifier. The porous member 37 is preferably designed to be gas permeable and liquid impervious. It can, in a preferred embodiment, be made of a buoyant material so that when the container is placed in a horizontal position, it tends to float on the top surface of the liquid layer, reducing the chance of liquid entrainment with the gas. Further, the container 4 can be operated horizontally by filling a container volume exceeding 50% with a liquid, preferably with a larger amount of liquid.

  In FIG. 4, the outlet port 12 is connected to the tube 35. The pipe | tube 35 gives the change of a flow direction to the gas delivered from a container. As the gas flows through the tube 35, droplets are deposited on the inner wall surface and removed from the gas. The tube shown in FIG. 4 allows the container to be operated horizontally with a container volume exceeding 50% filled with liquid. The tube 35 may impart one or more flow direction changes to the gas, such as a zigzag pattern with multiple flow changes. In addition to tube 35, other types of serpentine flow devices can be used, including filters, agglomeration filters, demister pads, porous media, and sintered media. The tube 35 can be connected to the valve 10 using a rotary joint 39. This joint can be rotated so that the end of the tube 35 communicates with the upper space 18 and not with the reactive liquid medium 6. A weight (not shown) can be used to ensure that the tube 35 is in the correct position and communicates with the upper space 18. A product gas purifier 9 can be added to the end of the tube 35 to prevent liquid from entering the tube 35. The product gas purifier 9 can include a membrane. Preferably, the membrane is positioned so that any liquid that contacts the membrane can be easily removed from the surface of the membrane.

FIG. 5 shows a diagram of the storage and delivery system 2 in a horizontal position with the valve 10 and outlet 12 attached. A membrane 38 is placed horizontally in the vessel 4 and serves as a gas / liquid separator as a particular embodiment of the product gas purifier 9. This membrane is made from a gas permeable, liquid impermeable material in order to be able to deliver gas from the container 4. Ideally, the membrane material repels the liquid so that it can be easily removed from its surface. Furthermore, to minimize pressure loss, the cross-sectional area of the membrane should be maximized and a microporous membrane (not a non-porous membrane) should be used. Suitable membrane materials include polytetrafluoroethylene (PTFE), polypropylene (PP), polyvinylidene fluoride (PVDF), polyethylene (PE), polysulfone, poly (vinyl chloride) PVC, rubber, poly (trimethylpentene), ethyl cellulose, Examples include poly (vinyl alcohol) (PVOH), perfluorosulfonic acid, polyethersulfone, cellulose ester, and polychlorotrifluoroethylene (PCTFE). A preferred pore size is 0.1 to 50 microns. In addition to using a thin film, the membrane can also consist of a thicker porous material, particularly one having a thickness of 10 millimeters or less. The membrane can also be a hollow fiber type membrane. (These same materials can also be used for the product gas purifier 9 of FIG. 1.) Gases suitable for storage and delivery from the storage and delivery system 2 described above have Lewis basicity. From a Lewis acid reactive liquid medium, such as an ionic liquid, or from a Lewis base reactive liquid medium having Lewis acidity. Lewis base gas is one of phosphine, arsine, stibine, ammonia, hydrogen sulfide, hydrogen selenide, hydrogen telluride, isotopically enriched analogues, basic organic or organometallic compounds, etc. Including the above. Gases with Lewis acidity that are stored in a Lewis base reactive liquid medium, such as an ionic liquid, and then delivered are diborane, boron trifluoride, boron trichloride, SiF ₄ , germane, hydrogen cyanide, HF, It includes one or more of HCl, HI, HBr, GeF ₄ , isotope-rich analogs, indium hydride, acidic organic or organometallic compounds, and the like. Additional gases such as disilane, digermanium, dialucine, and diphosphine may be suitable for storage and delivery with a reactive liquid medium. The liquid has a low volatility and preferably has a vapor pressure of less than about 10 ⁻² Torr at 25 ° C., more preferably less than 10 ⁻⁴ Torr at 25 ° C.

The ionic liquid can act as a reactive liquid for performing a reversible reaction with the gas to be stored, i.e., either a Lewis acid or a Lewis base. These reactive ionic liquids have a cation component and an anion component. As a result, the acidity or basicity of the reactive ionic liquid depends on the strength of the cation, anion, or the combination of cation and anion. The most common ionic liquids include salts of tetraalkylphosphonium, tetraalkylammonium, N-alkylpyridinium or N, N′-dialkylimidazolium cations. Common cations contain C _1-18 alkyl groups, and common cations include ethyl, butyl and hexyl derivatives of N-alkyl-N′-methylimidazolium and N-alkylpyridinium. Other cations include pyridazinium, pyrimidinium, pyrazinium, pyrazolium, triazolium, thiazolium, and oxazolium.

In order to achieve Lewis acidity, various anions can be partners of the cation component of such ionic liquids. One type of anion is derived from a metal halide. The most commonly used halide is chloride, but other halides can be used. Preferred metals for supplying anionic components, such as metal halides, include copper, aluminum, iron, zinc, tin, antimony, titanium, niobium, tantalum, gallium, and indium. Examples of metal chloride anions are CuCl ₂ ⁻ , Cu ₂ Cl ₃ ⁻ , AlCl ₄ ⁻ , Al ₂ Cl ₇ ⁻ , ZnCl ₃ ⁻ , ZnCl ₄ ²⁻ , Zn ₂ Cl ₅ ⁻ , FeCl ₃ ⁻ , FeCl ₄ ^−. Fe ₂ Cl ₇ ⁻ , TiCl ₅ ⁻ , TiCl ₆ ²⁻ , SnCl ₅ ⁻ , SnCl ₆ ²⁻ , and the like.

  Examples of halogen compounds from which Lewis acid or Lewis base ionic liquids can be prepared include 1-ethyl-3-methylimidazolium bromide, 1-ethyl-3-methylimidazolium chloride, 1-butyl-3-methyl. Imidazolium bromide, 1-butyl-3-methylimidazolium chloride, 1-hexyl-3-methylimidazolium bromide, 1-hexyl-3-methylimidazolium chloride, 1-methyl-3-octylimidazolium bromide, 1-hexyl Methyl-3-octylimidazolium chloride, monomethylamine hydrochloride, trimethylamine hydrochloride, tetraethylammonium chloride, tetramethylguanidine hydrochloride, N-methylpyridinium chloride, N-butyl-4-methylpyridinium bromide, N-butyl -4-methylpyridinium chloride, tetrabutylphosphonium chloride, and tetrabutylphosphonium bromide, and the like.

With respect to Lewis basic ionic liquids that are useful for chemically complexing Lewis acid gases, the anionic or cationic component or both of such ionic liquids can be Lewis bases. In some cases, both anions and cations are Lewis bases. Examples of Lewis base anions include carboxylate, fluorinated carboxylate, sulfonate, fluorinated sulfonate, imide, borate, chlorine (chloride), and the like. Common anion forms include BF ₄ ⁻ , PF ₆ ⁻ , AsF ₆ ⁻ , SbF ₆ ⁻ , CH ₃ COO ⁻ , CF ₃ COO ⁻ , CF ₃ SO ₃ ⁻ , p-CH ₃ —C ₆ H ₄ SO ^{_{3 -, (CF 3 SO 2}} ) 2 n -, (NC) 2 n -, (CF 3 SO 2) 3 C -, chloride (chloride), and F (HF) _n ^- and the like. Other anions include organometallic compounds such as alkyl aluminates, alkyl or aryl borates, as well as transition metal species. Preferred anions include BF ₄ ⁻ , p—CH ₃ —C ₆ H ₄ SO ₃ ⁻ , CF ₃ SO ₃ ⁻ , (CF ₃ SO ₂ ) ₂ N ⁻ , (NC) ₂ N ⁻ , (CF ₃ SO _{2 3} C ⁻ , CH ₃ COO ⁻ and CF ₃ COO ⁻ .

  Nonvolatile covalent liquids containing Lewis acid or Lewis base functional groups are also useful as reactive liquids for chemically complexing gases. Such liquids can be separate organic or organometallic compounds, oligomers, low molecular weight polymers, branched amorphous polymers, natural and synthetic oils, and the like.

  Examples of reactive liquids with Lewis acid functional groups include substituted boranes, borates, aluminum, or alumoxanes, protonic acids such as carboxylic acids and sulfonic acids, and complexes of metals such as titanium, nickel, copper, etc. , Etc.

  Examples of reactive liquids having a Lewis base functional group include ethers, amines, phosphines, ketones, aldehydes, nitriles, thioethers, alcohols, thiols, amides, esters, urea, carbamates, and the like.

  Specific examples of reactive covalent liquids include tributyl borane, tributyl borate, triethyl aluminum, methane sulfonic acid, trifluoromethane sulfonic acid, titanium tetrachloride, tetraethylene glycol dimethyl ether, trialkyl phosphine, trialkyl phosphine oxide, poly Examples include tetramethylene glycol, polyester, polycaprolactone, poly (olefin-alt-carbon monoxide), acrylate, methacrylate or acrylonitrile oligomer, polymer or copolymer. However, in many cases, these liquids suffer from excessive volatility at high temperatures and are not suitable for heat-mediated emissions. However, they may be suitable for pressure mediated release.

  As mentioned above, the gas delivered from the storage and delivery system 2 should be at least as pure as the source gas introduced into the container, and preferably the delivered gas is source gas Even more pure. However, when the gas is introduced into the container, impurities present in the raw material gas may be concentrated in the gas upper space on the reactive liquid medium. As a result, the gas initially withdrawn from the container may not be as pure as the source gas introduced into the container. In order to increase the purity of the feed gas from the storage and delivery system 2, the raw material gas exceeds the intended filling capacity of the container during the filling process, generally the reaction capacity of the reactive liquid medium. Can be introduced into the container. The intended fill volume is the amount of gas desired in the container at the end of the filling process. Next, the gas is removed from the container to remove impurities concentrated in the upper space. Residual gas in the container is used as product gas for delivery.

Furthermore, the source gas can be purified before it is introduced into the container. The source gas can be purified using adsorption purification, absorption purification, separation based on relative volatility difference, or reaction purification. Purification of the source gas is particularly effective when impurities in the source gas either react with the reactive liquid medium or dissolve in the reactive liquid medium. For example, in a system used to deliver and store BF _3, BF ₃ of the raw material may contain CO ₂ as an impurity. This impurity may react with or dissolve in a suitable reactive liquid medium. Adsorption purification can be used to remove this CO ₂ from the source gas. In particular, a bed of zeolite adsorbent and / or activated carbon adsorbent can be placed upstream of the vessel of reactive liquid medium. As the raw material BF ₃ passes through the zeolite bed, CO ₂ impurities are removed. The zeolite can be 5A zeolite or sodium mordenite zeolite.

1 is a cross-sectional view of a storage and delivery system containing a liquid that can react with a gas that uses a sparger tube to energize the storage and delivery system. 1 is a cross-sectional view of a storage and delivery system that incorporates heating and cooling mandrels to energize and / or remove energy from the system. FIG. 4 is a cross-sectional view of a storage and delivery system that uses a floating member at the end of a flexible tube to allow gas / liquid separation when the container is operated in either a vertical or horizontal position. FIG. 5 is a cross-sectional view of a storage and delivery system that uses a flexible flow path to allow gas / liquid separation when the container is operated in either a vertical or horizontal position. FIG. 3 is a cross-sectional view of a storage and delivery system that uses a longitudinally mounted member to allow gas / liquid separation when the container is operated in either a vertical or horizontal position.

Explanation of symbols

2 Gas storage and delivery system 4 Container 6 Reactive liquid medium 8 Gas 9 Product gas purifier 10 Valve 11 Inlet port 12 Outlet port 18 Upper space 28 Cooling mandrel 29 Heating mandrel 30 Stirrer 35 Tube 36 Flexible tube 37 Porous member 39 Rotary joint

Claims (24)

A container having an internal portion that contains a reactive Lewis base or Lewis acid reactive liquid medium that reversibly reacts with an opposite Lewis acidic or basic gas;
A valve system having an outlet port that enables gas delivery, and a product gas purifier,
Low pressure storage and delivery system for gas including.   The storage and delivery system of claim 1, wherein the product gas purifier is a gas / liquid separator.   The storage and delivery system of claim 1, wherein the product gas purifier is disposed within the vessel.   The storage and delivery system of claim 2, wherein the gas / liquid separator is comprised of a membrane.   The storage and delivery system according to claim 2, wherein the gas / liquid separator is composed of a member having a meandering passage through which an entrained liquid in the gas to be delivered can be agglomerated.   The storage and delivery system of claim 2, wherein the gas / liquid separator is comprised of a flexible tube that terminates in a floating porous member.   The storage and delivery system of claim 1, further comprising a bubble nucleation enhancer.   The storage and delivery system of claim 1, further comprising a source gas purifier.   The storage and delivery system of claim 1, wherein a purification medium is present in the reactive liquid medium.   The storage and delivery system of claim 9, wherein the purification medium is a chemical sorbent.   The reactive liquid medium is an ionic liquid, and the gas complexed with the ionic liquid comprises stibine, indium hydride, phosphine, boron trifluoride, isotope enriched boron trifluoride, germane and arsine. 2. A storage and delivery system according to claim 1 selected from the group. A container having an internal portion that contains a reactive Lewis base or Lewis acid reactive liquid medium that reversibly reacts with an opposite Lewis acidic or basic gas;
A valve system having an outlet port that allows gas delivery;
A system for transferring energy to or from a reactive liquid medium contained within the interior of the container;
Low pressure storage and delivery system for gas including.   The storage and delivery system of claim 12, wherein the valve has an inlet port.   The storage and delivery system of claim 12, wherein the system for charging energy to the reactive liquid medium comprises a sparger tube.   15. A storage and delivery system according to claim 14, wherein the sparger tube incorporates a porous frit.   13. A storage and delivery system according to claim 12, wherein the system for introducing energy into the reactive liquid medium comprises a stirrer for mixing the liquid.   13. A storage and delivery system according to claim 12, wherein the system for transferring energy consists of heating and / or cooling mandrels. A container having an internal portion that contains a reactive Lewis base or Lewis acid reactive liquid medium that reversibly reacts with an opposite Lewis acidic or basic gas;
A valve system having an inlet port for introduction of gas and reactive liquid medium into the vessel and an outlet port for gas delivery;
A system comprised of a sparger tube for introducing energy into the reactive liquid medium, and a gas / liquid separator that does not allow permeation of entrained droplets and permeation of gas when delivered from the vessel;
Low pressure storage and delivery system for gas including.   19. A storage and delivery system according to claim 18, wherein the gas / liquid separator is a tube having a tortuous passageway that allows agglomeration of entrained liquid in the gas to be delivered.   19. The storage and delivery system of claim 18, wherein the gas / liquid separator is a membrane. Put a reactive liquid medium of Lewis base or Lewis acid in a container with an internal part,
A raw material gas containing a Lewis base or Lewis acid reactive gas having the opposite Lewis acidity or basicity that reacts reversibly with the reactive liquid medium having Lewis acidity or basicity is placed in the container,
Collect excess unreacted source gas in the upper space of the vessel,
Drain the excess source gas from the upper space of the vessel to remove impurities concentrated in the upper space, and then
Delivering product gas,
A method for delivering product gas from a storage and delivery system comprising: Put a reactive liquid medium of Lewis base or Lewis acid in a container with an internal part,
A raw material gas containing a Lewis base or a Lewis acid reactive gas having the opposite Lewis acid or basicity that reversibly reacts with the reactive liquid medium having Lewis acidity or basicity is purified into the raw material gas. Remove any impurities present,
Introducing the refined source gas into a container,
And delivering product gas,
A method for delivering product gas from a storage and delivery system comprising:   23. The method of claim 22, wherein the reactive gas is boron trifluoride and the impurity is carbon dioxide.   24. The method of claim 23, wherein zeolite is used to remove carbon dioxide from boron trifluoride.

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